The objective of this thesis was to develop multi-responsive materials based on electro- and/or photoactive molecules. During this project, we synthesized and characterized three different π-conjugated molecules: naphthalene diimide-bridged silsesquioxane (NDI-PS), viologen-bridged silsesquioxane (VG-PS), and cationic naphthalene diimide (DaO). Organic/inorganic hybrid materials were obtained by polycondensation of organo-bridged trialkoxysilanes incorporating naphthalene diimide bridges (NDI-PS) and viologen bridges (VG-PS). The organo-bridged polysilsesquioxane gels exhibit interesting characteristics for numerous applications, particularly in photo-/electrochromic properties due to the presence of electroactive centers. To understand their properties and their relation to the structure of the 3D network, we explored different orthogonal synthetic routes to these gels, studying their influence on the organization of organic motifs within the network. Additionally, we investigated the photoinduced processes of discrete NDI-based derivatives, which were found to be associated with aggregation and/or radical generation depending on the NDI-based derivative and experimental conditions. VG-PS was utilized to prepare electrochromic films via electrodeposition. Furthermore, we demonstrated the incorporation of guest species of catalytic interest, such as iron(III) tetrasulfonate porphyrins, within these films.
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